Nanozymes have captured significant attention as a versatile and promising alternative to natural enzymes in catalytic applications, with wide-ranging implications for both diagnosis and therapy. However, the limited selectivity exhibited by many nanozymes presents challenges to their efficacy in diagnosis and raises concerns regarding their impact on the progression of disease treatments. In this article, we explore the latest innovations aimed at enhancing the selectivity of nanozymes, thereby expanding their applications in theranostic nanoplatforms. We place paramount importance on the critical development of highly selective nanozymes and present innovative strategies that have yielded remarkable outcomes in augmenting selectivities. The strategies encompass enhancements in analyte selectivity by incorporating recognition units, refining activity selectivity through the meticulous control of structural and elemental composition, integrating synergistic materials, fabricating selective nanomaterials, and comprehensively fine-tuning selectivity via approaches such as surface modification, cascade nanozyme systems, and manipulation of external stimuli. Additionally, we propose optimized approaches to propel the further advancement of these tailored nanozymes while considering the limitations associated with existing techniques. Our ultimate objective is to present a comprehensive solution that effectively addresses the limitations attributed to non-selective nanozymes, thus unlocking the full potential of these catalytic systems in the realm of theranostics. This work explores cutting-edge strategies to enhance nanozyme selectivity, vital for improving diagnostics and treatments, unlocking their full theranostic potential.